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In this work, quantum mechanical calculations and grand canonical Monte Carlo simulations were performed to study H2 and CH4 uptakes as well as CO2 separation from CH4 or H2 in MOF‐205 with different modification approaches. Upon C48B12 impregnation and Li decoration, B‐doped MOF‐205 shows remarkably improved gas adsorption and separation performances. Under ambient condition, both H2 and CH4 storage...
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